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2 CHEMICAL ENERGY STORAGE IC4 Cobalt supported catalysts exhibited catalytic properties similar to their nickel-based counterparts. The decision was therefore made to carry out comparative screening of the promoters used for both systems. The results showed that the promoting effects were similar for the two metals studied. Metal additives that lower the methane selectivity in favour of increased CO production always resulted in a reduction of activity compared with the un- promoted reference system. The PhotoCOO subproject was concerned with the elementary steps invol- ved in the aqueous reduction of CO2. In the case of the homogeneous cata- lysts, the research teams acquired a deeper understanding of the low tur- nover numbers caused by light-induced decomposition. A completely new photoreactor system using LED arrays was developed that provided light energy only for the required reaction channels. This work has identified an area with enormous development potential for new photostable catalysts as well as for new reactor systems. The goal of the team working at the Department of Chemical Technology II (TUM) was to develop a solar-powered single-stage route to C1 chemical buil- ding blocks and energy carriers from carbon dioxide and water using hetero- geneous photocatalysts. After successfully setting up a pilot plant to synthe- sise photo-semiconductors and after spectroscopically characterising them and studying their kinetics, experiments on the single-stage photocatalytic reduction of CO2 indicated that the reaction would proceed at a very low rate due to the large overpotentials present. To overcome these kinetic barriers, a two-stage process was developed in which the generation of hydrogen and the subsequent hydrogenation of carbon dioxide were decoupled in time. The photocatalytic generation of hydrogen can occur by the photoreforming of wastewater containing polyols or through a water-splitting reaction. Detailed studies of the anodic reaction network of the C2- and C3-polyol reforming reaction to carbon dioxide showed that the oxidation step and the C-C bond cleavage occurred via the same reaction mechanism. In this reaction, formal- dehyde accumulates in the liquid phase due to the small adsorption constant and is then oxidised to formic acid as soon as the more strongly adsorbing in- termediates (glycolaldehyde or formic acid) have been converted. In a collaborative project with the Krischer and Rieger groups, silicon-based semiconductor surfaces were modified with nitrogen-containing organic residues (pyridines) in such a way that the CO2 is absorbed from the aqueous phase so that electron transfer can occur from the surface to the bound CO2. These organomodified surfaces exhibited a significantly greater electroche- mical activity for hydrogen generation and for the reduction of CO2 to met- hanol and showed themselves to be both chemically and electrochemically stable. The reaction mechanism of the reduction of CO2 on platinum elec- 158PDF Image | Chemical Processes and Use of CO2
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